Authors
Aruna Kumarasiri, Amin Yousefi, Dennis Hore
Published in
The Journal of chemical physics. Volume 165. Issue 15. Oct 21, 2026.
Abstract
The structure of molecules at surfaces and buried interfaces can be probed by second-order nonlinear optical techniques that derive their response from environments with broken centrosymmetry, thereby simultaneously enhancing the signal from the molecules of interest and suppressing the responses of the adjacent bulk phases. However, even though these methods are surface-sensitive, extracting orientation information has often relied on significant assumptions about the shape of the orientation distribution and the underlying molecular electronic structure. Here, we illustrate that the measurement of the relative magnitude and the phase of tensor elements that govern the vibrational sum frequency response can be used to construct a ratio of order parameters ⟨P3⟩/⟨P1⟩. This structural parameter does not require knowledge of the hyperpolarizability or even the hyperpolarizability ratio, thereby dramatically increasing the accuracy of its determination. We then show how this parameter can be used to comment on the most probable distribution of tilt angles. This is demonstrated for para-cyanophenol at three different interfaces.
PMID:
42895429
Bibliographic data and abstract were imported from PubMed on 19 Oct 2026.
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